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弱亲水性亚胺键联共价苯乙炔骨架在两相体系中光催化 HO 生成。

Weakly Hydrophilic Imine-Linked Covalent Benzene-Acetylene Frameworks for Photocatalytic HO Production in the Two-Phase System.

机构信息

School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200241, P. R. China.

出版信息

ACS Appl Mater Interfaces. 2023 Feb 15;15(6):8066-8075. doi: 10.1021/acsami.2c20506. Epub 2023 Feb 1.

Abstract

Conversing oxygen (O) to hydrogen peroxide (HO) driven by solar energy is a promising HO onsite production route but often short of efficient and durable photocatalysts. Herein, strong π-π conjugate polycyclic aromatic benzene and acetylene units have been constructed into new covalent organic frameworks (COFs) linked by imine C═N bonding. These COFs demonstrated two-dimensional hexagonal crystalline frameworks with higher crystallinity and larger surface area (>600 m g). Covalent benzene-acetylene frameworks possessed appropriate visible light-responsive band structure and the suppressed charge recombination rate. The -OH groups on their frameworks enable them to be weakly hydrophilic. As a result, it served as high-performance but durable photocatalysts for HO production in the water-benzyl alcohol (BA) two-phase system. It delivered a HO production rate of 1240 μmol h g and durable catalytic efficiency within 60 h, comparable to the best COF-based catalysts. This study provides an efficient two-phase photocatalytic system for HO production based on weakly hydrophilic imine-linked benzene-acetylene organic photocatalysts.

摘要

受太阳能驱动,将氧气(O)转化为过氧化氢(HO)是一种很有前景的 HO 现场生产途径,但往往缺乏高效和耐用的光催化剂。在此,强π-π共轭多环芳烃和乙炔单元已被构建成新的共价有机框架(COFs),通过亚胺 C═N 键连接。这些 COFs 表现出具有更高结晶度和更大表面积(>600 m g)的二维六方晶状结构。共价苯-乙炔框架具有合适的可见光响应能带结构和抑制的电荷复合率。其框架上的-OH 基团使它们具有较弱的亲水性。结果,它们作为高性能但耐用的光催化剂,用于水-苄醇(BA)两相体系中的 HO 生产。它在 60 h 内实现了 1240 μmol h g 的 HO 生成速率和持久的催化效率,可与最佳的基于 COF 的催化剂相媲美。本研究为基于弱亲水亚胺连接的苯-乙炔有机光催化剂的 HO 生产提供了高效的两相光催化系统。

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